Carbonaceous aerosol transport from the Indo-Gangetic Plain to the Himalayas: Carbon isotope evidence and light absorption characteristics

The Indo-Gangetic Plain (IGP) is a major regional and global emitter of atmospheric pollutants, which adversely affect surrounding areas such as the Himalayas. We present a comprehensive dataset on carbonaceous aerosol (CA) composition, radiocarbon (Δ¹⁴C) -based source apportionment, and light absorption of total suspended particle (TSP) samples collected over a 3-year period from high-altitude Jomsom in the central Himalayas. The 3-year mean TSP, organic carbon (OC), and elemental carbon (EC) concentrations were 92.0 ± 28.6, 9.74 ± 6.31, and 2.02 ± 1.35 μg m^?3, respectively, with the highest concentrations observed during the pre-monsoon season, followed by the post-monsoon, winter, and monsoon seasons. The Δ¹⁴C analysis revealed that the contribution of fossil fuel combustion (f_fossil) to EC was 47.9% ± 11.5%, which is consistent with observations in urban and remote regions in South Asia and attests that EC likely arrives in Jomsom from upwind IGP sources via long-range transport. In addition, the lowest f_fossil (38.7% ± 13.3%) was observed in winter, indicating large contributions in this season from local biomass burning. The mass absorption cross-section of EC (MAC_EC: 8.27 ± 1.76 m²/g) and water-soluble organic carbon (MAC_WSOC: 0.98 ± 0.45 m²/g) were slightly higher and lower than those reported in urban regions, respectively, indicating that CA undergo an aging process. Organic aerosol coating during transport and variation of biomass burning probably led to the seasonal variation in MAC of two components. Overall, WSOC contributed considerably to the light absorption (11.1% ± 4.23%) of EC. The findings suggest that to protect glaciers of the Himalayas from pollution-related melting, it is essential to mitigate emissions from the IGP.     

Recent Progress of Aerosol Light-scattering Enhancement Factor Studies in China

Assessment of the radiative forcing of aerosols in models still lacks sufficient input data for aerosol hygroscopicity. The light scattering enhancement factor [ f(RH, λ)] is a crucial parameter for describing aerosol hygroscopic growth properties.In this paper, we provide a survey of f(RH, λ) studies in China for the past seven years, including instrument developments of humidified nephelometers, ambient f(RH, λ) measurements in China, f(RH, λ) parameterization schemes, and f(RH, λ)applications in aerosol measurements. Comparisons of different f(RH, λ) parameterizations are carried out to check their performance in China using field measurement datasets. We also summary the parameterization schemes for predicting f(RH, λ)with aerosol chemical compositions. The recently developed methods to observe other aerosol properties using f(RH, λ)measurements, such as calculating the aerosol hygroscopicity parameter, cloud condensation nuclei number concentration,aerosol liquid water content, and aerosol asymmetry factor, are introduced. Suggestions for further research on f(RH, λ) in China are given.     

Analysis of Low-level Temperature Inversions and Their Effects on Aerosols in the Lower Atmosphere

High-quality and continuous radiosonde, aerosol and surface meteorology datasets are used to investigate the statistical characteristics of meteorological parameters and their effects on aerosols. The data were collected at the Atmospheric Radiation Measurement Southern Great Plains climate research facility during 2000–15. The parameters and vertical distribution of temperature inversion layers were found to have strong diurnal and seasonal changes. For surface-based temperature inversion (SBI), the mean frequency and depth of temperature inversion layers were 39.4% and 198 m, respectively. The temperature difference between the top and bottom of SBI was 4.8℃, and so the temperature gradient was 2.4℃ (100 m)^?1. The detailed vertical distributions of temperature inversion had been determined, and only the temperature inversion layers below 1000 m showed diurnal and seasonal variations. Mean surface aerosol number concentrations increased by 43.0%, 21.9% and 49.2% when SBIs were present at 0530, 1730 and 2330 LST, respectively. The effect of SBI on surface aerosol concentration was weakest in summer (18.1%) and strongest in winter (58.4%). During elevated temperature inversion events, there was no noticeable difference in surface aerosol number concentrations. Temperature differences and temperature gradients across SBIs correlated fairly well with aerosol number concentrations, especially for temperature gradients. The vertical distribution of aerosol optical properties with and without temperature inversions was different. Surface aerosol measurements were representative of the air within (below), but not above, SBIs and EIs. These results provide a basis for developing a boundary layer aerosol accumulation model and for improving radiative transfer models in the lower atmosphere.     

石家庄地区2005年秋季污染气溶胶飞机观测资料分析

利用河北省2005年10月份的3次气溶胶飞机观测资料和宏观天气资料,综合分析石家庄地区不同天气条件下气溶胶的垂直分布和尺度谱分布特征。分析结果表明:气溶胶浓度的分布与大气环境情况密切相关。气溶胶数浓度最大值的变化范围是103~104cm-3,平均数浓度为103cm-3,粒子平均直径为0.120~0.150μm;21日近地面有霾,相对湿度为58%,近地面气溶胶浓度较17和29日略低,但粒子平均直径(0.165μm)比其余两次要大,可见相对湿度较大,大气中水汽含量较多,有利于小粒子凝结水汽,使粒子直径增大;逆温层结下,粒子在逆温层下累积,无逆温时数浓度最大值出现在近地面附近。气溶胶粒子谱呈单峰分布。     

夏季东亚地区AOD与地面太阳辐射变化的联系及季风环流异常:季节趋势影响

利用2000—2013年MODIS-Terra卫星产品提供的气溶胶光学厚度(aerosol optical depth,AOD)资料及NCEP/NCAR再分析资料集,使用奇异值分解(singular value decomposition,SVD)方法,分析了夏季东亚地区AOD与到达地面太阳辐射(downward solar radiation flux,DSRF)相联系的主要模态,并分析了其与夏季风变化的关系。夏季多年平均的AOD分布显示,在东亚地区存在两个AOD大值区(0.9),分别位于山东、河南、河北交界处附近以及苏中部分地区。而在福建、台湾及其附近洋面上,夏季AOD的值小于0.4。地面太阳辐射总体上呈现出由南往北递增的分布。比较发现,AOD与地面太阳辐射的气候分布较为相似。在保留季节趋势的情况下,运用SVD方法对两者进行分解,结果表明东亚地区AOD与地面太阳辐射表现出较好的正相关关系。由于相对于年际变化而言,季节趋势是更为主要的部分,因而这种同相关系可归因于季风活动的季节性进程。利用SVD1左场时间系数进行相关分析发现:6月(2013年除外),当中国东部气溶胶AOD大而地面太阳辐射亦大时,在中国东南部以及日本岛南部地区,由于气流辐合增强和存在较强的上升运动,降水偏多,而由于副高位置偏南,使得中国中东部偏北地区水汽供应偏弱,降水偏少。由于地面净太阳辐射增强,华北部分地区异常增暖。8月,大陆上空AOD为负(时间系数为负),地面太阳辐射减少,北方降水增多而南方降水减少,华北地区有一小范围的异常降温。上述结果表明北方气溶胶明显偏少时,云量增加,降水将增多,且辐射明显减弱;说明夏季风的季节进程对气溶胶、到达地面的太阳辐射变化等具有重要影响。     

霾期间上海低层气溶胶微物理属性与地面相对湿度分析

用2007年1月至2010年11月美国国家航空航天局(NASA)的CALIPSO星载激光雷达资料,通过532 nm总后向散射系数、体积退偏比和色比,分析了上海地区霾期间低层0~2 km高度气溶胶微物理属性与地面相对湿度的关系。结果表明,当地面相对湿度为65%~80%时,后向散射系数在0~0.001 km-1·sr-1范围内出现的频率最大;当地面相对湿度为50%~65%时,后向散射系数大于0.001 km-1·sr-1的频率最大;低层大气中聚集的主要是规则气溶胶粒子,当地面相对湿度为65%~80%时,气溶胶粒子最为规则,其次为80%~95%的地面相对湿度。当地面相对湿度为50%~65%时,不规则气溶胶粒子所占比重较大;霾期间,低层大气中细粒子气溶胶均占主导地位,但随着地面相对湿度的增大,气溶胶粒子粒径逐渐增大。在地面相对湿度为80%~95%时,大颗粒气溶胶相对较多。     

动态气溶胶模型的PARASOL多角度偏振卫星气溶胶光学厚度反演算法

在卫星气溶胶反演中,如何确定研究区域的气溶胶模型直接影响目前大多数卫星遥感算法的气溶胶光学厚度反演精度。本文基于气溶胶自动观测网(AERONET)典型类型的动态气溶胶模型,提出了一种基于动态气溶胶模型的气溶胶光学厚度反演算法,并将其运用到PARASOL(Polarization and Anisotropy of Reflectance for Atmospheric Science coupled with Observations from Lidar)卫星的反演中。针对华北地区2012年的PARASOL卫星观测数据,应用动态气溶胶模型反演算法反演气溶胶光学厚度,并与地面观测站点进行对比验证,结果显示通过气溶胶模型选取与反演结果的迭代约束,在865 nm反演的气溶胶光学厚度与地基观测的相关程度(R2)达到0.71,均方根误差(RMSE)为0.15,与PARASOL气溶胶产品相比一定程度提高了反演结果的精度。     

利用暗目标法从高分一号卫星16 m相机数据反演气溶胶光学厚度

针对高分一号卫星(GF-1)的16 m宽覆盖相机数据,探讨了暗目标法的应用。首先,利用地面观测的植被光谱数据,结合模拟计算,发现利用红蓝波段线性关系能更好地去除地表影响,而利用反演的气溶胶光学厚度AOD进行大气校正能很好地去除伪暗目标;然后,以天津地区和北京地区为试验区进行了反演试验。结果表明,利用本算法能较好地观测气溶胶分布,与地面观测结果均有较好的相关性(R0.8),但反演结果整体偏高,可能是云像元的影响。误差分析表明,整景图像采用统一的观测天顶角会带来较大误差,最大误差为0.3;绝对辐射定标精度在3%以下,反演精度能控制在10%,城市型气溶胶会对反演带来较大误差。     

塔克拉玛干沙漠腹地沙尘气溶胶质量浓度垂直分布特征

 利用Grimm 1.108、Thermo RP 1 400 a以及TSP等仪器于2009年1月至2010年2月对塔克拉玛干沙漠腹地塔中不同高度沙尘气溶胶质量浓度进行连续观测,结合天气资料进行分析。结果表明:①80 m高度PM10质量浓度最高,80 m高度PM2.5和PM1.0质量浓度明显低于4 m高度PM10,80 m高度PM1.0质量浓度最低。频繁的沙尘天气是影响不同粒径的沙尘气溶胶浓度含量的主要因素。②夜间至日出,PM质量浓度逐渐降低,最低基本上出现在08:00,随后质量浓度逐渐增大,18:00前后浓度达到最高值,然后又逐步降低。其规律与风速的昼夜变化完全一致。③TSP月平均质量浓度高值主要集中在3—9月,其中4月和5月浓度最高,随后逐渐减低。3—9月也是PM月平均质量浓度的高值区域,4 m高度PM10月平均质量浓度最高发生在5月,其浓度为846.0 μg·m-3。80 m高度PM10浓度远高于PM2.5和PM1.0浓度,PM2.5和PM1.0浓度相差较小。风沙天气对大气中的不同粒径粒子的浓度含量影响较大,风沙天气越多,粗颗粒含量越高,反之则细颗粒越多。④沙尘天气过程中不同粒径沙尘气溶胶质量浓度变化具有晴天<浮尘天气<扬沙天气<沙尘暴天气的规律。各种沙尘天气中,PM10/TSP表现为晴好天气高于浮尘天气,浮尘天气远高于扬沙和沙尘暴天气。⑤沙尘天气过程中,沙尘气溶胶浓度随着粒径的减小,浓度逐渐降低。不同高度、不同粒径的沙尘气溶胶质量浓度每隔3~4 d形成一个峰值区,与每隔3~4 d出现沙尘天气强度增强过程直接相关。     

A review of global stratospheric aerosol: Measurements, importance, life cycle, and local stratospheric aerosol

Stratospheric aerosol, noted after large volcanic eruptions since at least the late 1800s, were first measured in the late 1950s, with the modern continuous record beginning in the 1970s. Stratospheric aerosol, both volcanic and non-volcanic are sulfuric acid droplets with radii (concentrations) on the order of 0.1–0.5 µm (0.5–0.005 cm^− 3), increasing by factors of 2–4 (10–10³) after large volcanic eruptions. The source of the sulfur for the aerosol is either through direct injection from sulfur-rich volcanic eruptions, or from tropical injection of tropospheric air containing OCS, SO₂, and sulfate particles. The life cycle of non-volcanic stratospheric aerosol, consisting of photo-dissociation and oxidation of sulfur source gases, nucleation/condensation in the tropics, transport pole-ward and downward in the global planetary wave driven tropical pump, leads to a quasi steady state relative maximum in particle number concentration at around 20 km in the mid latitudes. Stratospheric aerosol have significant impacts on the Earth's radiation balance for several years following volcanic eruptions. Away from large eruptions, the direct radiation impact is small and well characterized; however, these particles also may play a role in the nucleation of near tropopause cirrus, and thus indirectly affect radiation. Stratospheric aerosol play a larger role in the chemical, particularly ozone, balance of the stratosphere. In the mid latitudes they interact with both nitrous oxides and chlorine reservoirs, thus indirectly affecting ozone. In the polar regions they provide condensation sites for polar stratospheric clouds which then provide the surfaces necessary to convert inactive to active chlorine leading to polar ozone loss. Until the mid 1990s the modern record has been dominated by three large sulfur-rich eruptions: Fuego (1974), El Chichón (1982) and Pinatubo (1991), thus definitive conclusions concerning the trend of non-volcanic stratospheric aerosol could only recently be made. Although anthropogenic emissions of SO₂ have changed somewhat over the past 30 years, the measurements during volcanically quiescent periods indicate no long term trend in non-volcanic stratospheric aerosol.